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21.
We employ density functional and quantum Monte Carlo calculations to show that significant changes occur in the gap of fully hydrogenated nanoclusters when the surface contains passivants other than hydrogen, in particular atomic oxygen. In the case of oxygen, the gap reduction computed as a function of the nanocluster size provides a consistent interpretation of several recent experiments. Furthermore, we predict that other double bonded groups also significantly affect the optical gap, while single bonded groups have a minimal influence.  相似文献   
22.
Remmel  Jeffrey B.  Williamson  S. Gill 《Order》1999,16(3):245-260
Let N denote the set of natural numbers and let P =(N k , ) be a countably infinite poset on the k-dimensional lattice N k . Given x N k , we write max(x) (min(x)) for the maximum (minimum) coordinate of x. Let be the directed-incomparability graph of P which is defined to be the graph with vertex set equal to N k and edge set equal to the set of all (x, y) such that max(x) max(y) and x and y not comparable in P. For any subset D N k , we let P D and D denote the restrictions of P and to D. Points x N k with min(x) = 0 will be called boundary points. We define a geometrically natural notion of when a point is interior to P or relative to the lattice N k , and an analogous notion of monotone interior with respect to or D . We wish to identify situations where most of these interior points are exposed to the boundary of the lattice or, in the case of monotone interior points, not concealed very much from the boundary. All of these ideas restrict to finite sublattices F k and/or infinite sublattices E k of N k . Our main result shows that for any poset P and any arbitarily large integer M > 0, there is an F E with F = M where, relative to the sublattices F k E k , the ideal situation of total exposure of interior points and very little concealment of monotone interior points must occur. Precisely, we prove that for any P =(N k , ) and any integer M > 0, there is an infinite E N and a finite D F k with F E and F = M such that (1) every interior vertex of P E k or E k is exposed and (2) there is a fixed set C E, C k k , such that every monotone-interior point of D belonging to F k has its monotone concealment in the set C. In addition, we show that if P 1 =(N k , 1),..., P r =(N k , r ) is any sequence of posets, then we can find E,D, and F so that the properties (1) and (2) described above hold simultaneously for each P i . We note that the main point of (2) is that the bound k k depends only on the dimension of the lattice and not on the poset P. Statement (1) is derived from classical Ramsey theory while (2) is derived from a recent powerful extension of Ramsey theory due to H. Friedman and shown by Friedman to be independent of ZFC, the usual axioms of set theory. The fact that our result is proved as a corollary to a combinatorial theorem that is known to be independent of the usual axioms of mathematics does not, of course, mean that it cannot be proved using ZFC (we just couldn"t find such a proof). This puts our geometrically natural combinatorial result in a somewhat unusual position with regard to the axioms of mathematics.  相似文献   
23.
24.
The 13C NMR spectra of four pairs of 1,3,4-thiadiazole/thiadiazoline isomers have been recorded using broad band and off-resonance proton decoupling techniques and in the coupled mode. Differences in the chemical shifts of the heterocyclic ring and the carbonyl carbons allow identification of the isomer present. Their IR and UV spectra are in agreement with literature reports for azole/azoline analogues.  相似文献   
25.
26.
The EPR spectrum of O on MgO has been observed following the reaction of N2O with electrons trapped at the surface. The spectrum of the ion in axial symmetry is characterized by g = 2.041 and g = 2.0016. Upon exposure to H2, CO, CO2 or additional N2O the spectrum is replaced by another having g1 = 2.0172, g2 = 2.0100 and g3 = 2.0014. This spectrum is tentatively assigned to the O3 ion.  相似文献   
27.
The effect of preparation conditions on the structural and optical properties of silicon nanoparticles is investigated. Nanoscale reconstructions, unique to curved nanosurfaces, are presented for silicon nanocrystals and shown to have lower energy and larger optical gaps than bulk-derived structures. We find that high-temperature synthesis processes can produce metastable noncrystalline nanostructures with different core structures than bulk-derived crystalline clusters. The type of core structure that forms from a given synthesis process may depend on the passivation mechanism and time scale. The effect of oxygen on the optical of different types of silicon structures is calculated. In contrast to the behavior of bulklike nanostructures, for noncrystalline and reconstructed crystalline structures surface oxygen atoms do not decrease the gap. In some cases, the presence of oxygen atoms at the nanocluster surface can significantly increase the optical absorption gap, due to decreased angular distortion of the silicon bonds. The relationship between strain and the optical gap in silicon nanoclusters is discussed.  相似文献   
28.
Glucosinolates (GLSs) are relatively inert (Z)-N-hydroximinosulfate esters, possessing a sulfur-linked beta-D-glucopyranose moiety and a variable side chain, found almost exclusively in cruciferous vegetables. Following cell disruption, they are hydrolysed by plant myrosinases, forming a group of chemically reactive and biologically active compounds. There is considerable evidence that these breakdown products, when consumed in the diet, may affect the risk of developing chronic diseases. However, in order for any compound to exert an activity in vivo, it is necessary to reach the site of action in an appropriate form and sufficient concentration. Deleterious and toxic effects may be observed at high concentrations: hence, bioavailability is a key factor defining the physiological, beneficial dose window of GLS hydrolysis products (GLS-HPs). For some GLS-HPs, this window can be rather narrow, and therefore is a critical parameter to be considered. In this review we critically evaluate the present state of knowledge on all factors that affect bioavailability of GLS-HPs. This includes liberation from the plant material, absorption from the digestive system, distribution around the body, metabolism and excretion.  相似文献   
29.
We present density functional and quantum Monte Carlo calculations of the stability and optical properties of semiconductor nanomaterials with reconstructed surfaces. We predict the relative stability of silicon nanostructures with reconstructed and unreconstructed surfaces, and we show that surface step geometries unique to highly curved surfaces dramatically reduce the optical gaps and decrease excitonic lifetimes. These predictions provide an explanation of both the variations in the photoluminescence spectra of colloidally synthesized nanoparticles and observed deep gap levels in porous silicon.  相似文献   
30.
In controlled N-nutrition experiments, differences in delta15N composition of leaves and roots are regularly found. In this paper we report results from a survey of nitrogen stable isotope signatures of leaves and roots of 16 plant species growing under natural conditions in a meadow and a forest understorey, which differed in nitrate and ammonium availability. Significant differences between leaf and root were observed. The range of delta15N [leaf-root] values was -0.97 to +0.86 per thousand, small compared to published values from controlled N-nutrition experiment, but almost as large as the range of leaf delta15N values (-1.04 to +1.08 per thousand). Forbs showed the largest differences between leaves and roots and showed a significant difference with respect to habitat. Grasses and legumes did not show significant differences in delta15N [leaf-root] between the two habitats. Care must be taken when using leaf delta15N values as representative for whole-plant 15N composition in these two habitats.  相似文献   
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